effect of sheep manure and edta on the leaching of potassium from heavy metals contaminated...
TRANSCRIPT
ORIGINAL ARTICLE
Effect of sheep manure and EDTA on the leaching of potassiumfrom heavy metals contaminated calcareous soils
M. Jalali • H. Ostovarzadeh
Received: 1 September 2010 / Accepted: 4 July 2011 / Published online: 26 July 2011
� Springer-Verlag 2011
Abstract In this study, we examined the movement of
potassium (K) in columns of contaminated calcareous soils
by sheep manure and ethylene diamine tetraacetic acid
(EDTA). Glass tubes, 4.9 cm in diameter and 40 cm in
length, were packed with contaminated soils. The resulting
20-cm long column of soil had a bulk density of
1.3–1.4 g cm-3. Columns were leached with distilled
water, 0.01 M EDTA, 0.01 M CaCl2, and sheep manure
extract solutions. The amounts of K leached varied con-
siderably between different soils (sandy loam and loamy
sand) and leaching solutions. The amount leached with
EDTA solution, varied from 7.2 to 66.7% of the extract-
able K when 20 pore volumes had passed through the
column. The breakthrough curves of K in the EDTA and
CaCl2 were approximately similar, indicating they have
similar ability to displace K from these contaminated
calcareous soils. Thus, among leaching solutions applica-
tion of EDTA and CaCl2 on contaminated soils might
enhance the mobility of K and large amounts of K will be
leached.
Keywords Leaching � Calcareous soils � Potassium �Sheep manure � EDTA
Introduction
Excessive application of chemical fertilizer in agricultural
soils had caused serious environmental problems in Iran.
Livestock and poultry manure can be an alternative source
of chemical fertilizer. The increasing sheep and poultry
industry in Iran, especially in the Hamedan province,
produces large amounts of sheep and poultry litter which
are used to enhance soil fertility (Jalali and Khanboluki
2007). In vegetable and field crops in the studied areas, the
use of organic manure (in potato fields about 10 t ha-1 is
being used) is common (Jalali 2005). Besides supplying
nutrients, organic litter affects metal solubility (del Casti-
lho et al. 1993). Dissolved organic matter in sheep manure
could contribute effectively organic ligands to form com-
plexes with heavy metals (Mc Bride 1989; Bolton et al.
1993) and other cations in soil.
Soil contamination with heavy metals due to the appli-
cation of sewage sludge, fertilizers, and industrial activities
is growing in Hamedan, western Iran. The growing rate of
industrialization in this area causes a high anthropogenic
emission of heavy metals from metal mining and smelting
activities, disposal of industrial wastes and application of
fertilizers and pesticides into the soil (Jalali and Khanlari
2008).
Potassium (K) is an essential macronutrient required by
plants for proper function. The fate of the K in arid and
semi-arid regions has received less attention than that of
nitrogen or phosphorus and little attention has been given
to K leaching because K does not result directly in eutro-
phication (Alfaro et al. 2004). Potassium leaching is
affected by soil texture, available K, drying and wetting,
and types of other cations present in the soil solution
(Evangelou and Lumbaraja 2002; Kolahchi and Jalali
2007), among other factors. Rosolem et al. (2010) studied
the effects of soil texture and K availability on K leaching.
They found that K leaching below the arable layer
increased with K rates, but the effect was less noticeable in
the clay soil. The effects of four fertilizer regimes on the
nutrient balances and leaching of K from grassland grown
M. Jalali (&) � H. Ostovarzadeh
Department of Soil Science, College of Agriculture,
Bu-Ali Sina University, Hamedan, Iran
e-mail: [email protected]
123
Environ Earth Sci (2012) 66:31–37
DOI 10.1007/s12665-011-1200-z
on a sandy soil were investigated by Kayser et al. (2007).
They found that high levels of exchangeable K in the soil
and/or large rate fertilizer or urine applications increased
leaching of K. Jalali and Ranjbar (2009) studied the effect
of gypsum application on K leaching under unsaturated
steady state flow conditions in undisturbed soil columns.
They concluded that the use of sources of water for irri-
gation which have a high Ca concentration can lead to
leaching of K from soil. Alfaro et al. (2004) performed an
experiment to understand the effects of N and farmyard
manure on the dynamics of K leaching on a hillslope
grassland soil in southwestern England. Higher total K
losses and K concentrations in the leachates were found in
the nitrogen and farmyard manure treatments, which were
related to K additions in the farmyard manure. Ground-
water K contamination can result from application of
inorganic fertilizer at greater than agronomic rates. Losses
of nutrients, including K, from agricultural land have been
identified as one of the main causative factors in reducing
water quality in many parts of arid and semi-arid regions
(Griffioen 2001; Kolahchi and Jalali 2007). Recent survey
of well water quality in Chah basin, western Iran indicated
that the K concentrations in water samples ranged between
0.12 and 63 mg l-1 and 9% of rural wells have K con-
centrations in excess of drinking water guidelines
(12 mg l-1) (Griffioen 2001; WHO 1993), in regions with
high-demand crops (Jalali 2007). Irrigation with water
having high concentrations of Ca, Mg and Na leads to an
increase in K desorption and leaching (Jalali et al. 2008).
Ethylene diamine tetraacetic acid (EDTA) is commonly
used chelate in soil science for different purposes such as
prediction of the bioavailability of heavy metals (Chen
et al. 2004; Alvarez et al. 2006), supplying micronutrient
cations for plants (Manouchehri et al. 2006; Alvarez et al.
2006) and soil remediation processes (Brown and Elliot
1992; Pichtel and Pichtel 1997; Sun et al. 2001; Finzgar
and Lestan 2007). Adding soluble organic ligands such as
sheep manure has been reported to reduce the sorption of
heavy metals by soils (Shuman 1995). Application of
EDTA and sheep manure extract (SME) solution in recla-
mation of contaminated soils may also cause leaching of
nutrients, including K. Jalali and Ostovarzadeh (2009)
studied P leaching from contaminated calcareous soils due
to the application of SME and EDTA. They found that
among leaching solutions the application of EDTA and
SME on contaminated calcareous soils might enhance the
mobility of P and large amounts of P will be leached,
leading to deterioration of ground and surface waters.
Around the world several studies have evaluated
leaching of K (Heming and Rowell 1997; Hombunaka and
Rowell 2002; Jalali and Rowell 2003; Alfaro et al. 2004;
Kolahchi and Jalali 2007), but experimental data on K
leaching losses from contaminated calcareous soils due to
application of sheep manure and EDTA are few.
Thus, to better understand K leaching by sheep manure
and EDTA and its contribution to poor water quality, soil
columns were employed to investigate the movement of K
in some contaminated calcareous soils ranging from low to
excessive in extractable K. Because cation exchange is the
most important mechanisms that affect K leaching, CaCl2was used as exchange-solution.
Materials and methods
The description of study area and soil sampling
Hamedan province is located in western Iran and lies
between longitudes 47�340 and 49�360 E and latitudes
33�580 and 35�480 N, with a history of more than
3,000 years and about 1.75 million inhabitants. The climate
of the study area is considered to be semi-arid, the annual
precipitation is approximately 300 mm. Rainfall occurs
from October to May, with a maximum during November
and February of each year. The mean monthly temperatures
vary between -4 and 25�C, and the mean annual value is
11�C. Farmland is a major industry and principal land use
in Hamedan province. The vegetation cover along the study
sites is dominated by annual and perennial plants, where
the most common are: Astragalus spp., Stipa barbata Desf,
Euphorbia Aellenii Rech. F., Lepidium latifolium L.,
Cheniopodium botrys L., Chenopodium murale L., Acan-
tholimon Festucaceum Boiss., Phlomis orientalis Mill.,
Centaurea spp, Achillea setacea Waldst. and Kit., and
Alhagi camelorum Fich (Jalali and Khanlari 2008). The
soils of the area are mostly classified as Entisols and
Inceptisols. The parent rocks are mainly limestone, cal-
careous shale and granitic material. Four sites located in
Hamedan province were investigated for the leaching
experiment. The soils were collected from four industrial
and mining sites (Jalali and Ostovarzadeh 2009). Soils
were air-dried and ground to pass through a 2-mm sieve.
Soil pH and electrical conductivity (EC) were measured in
H2O using a 1:5 soil to solution ratio, after the soil sus-
pension had been equilibrated at 25�C for 1 h on a shaker
(Rowell 1994). Particle size distribution was determined by
the hydrometer method. Organic matter (OM) was deter-
mined by dichromate oxidation (Rowell 1994). Calcium
carbonate equivalent (CCE) by neutralization with HCl,
cation exchange capacity (CEC) by replacing exchangeable
cations by NaOAc, and exchanging Na with NH4OAc
Rowell (1994). Extractable K was extracted using NH4OAc
Rowell (1994). Total heavy metals were measured using
4 M HNO3 for 12 h (Sposito et al. 1983).
32 Environ Earth Sci (2012) 66:31–37
123
Selected chemical and physical properties of the soils
are given in Jalali and Ostovarzadeh (2009). Clay contents
ranged from 80 to 284 g kg-1, CEC ranged from 17.0 to
21.3 cmolc kg-1, and organic carbon contents were low in
all samples ranging from 0.2 to 14.9 g kg-1. The soils were
neutral to alkaline and low in soluble salt content (EC
0.27–0.78 dS m-1). The NH4OAc extractable K ranged
from 420 to 920 mg kg-1. Based on the rating procedure of
Rowell (1994), three soils fall in the four indices
(401–600 mg K kg-1), and the content of K in one soil is
higher than this limit. The total Zn, Cd, Ni, Cu and Pb are
given in Jalali and Ostovarzadeh (2009). In conclusion, the
surface soils of studied area appeared to be contaminated in
the order by Pb [ Cd [ Zn [ Cu [ Ni (Jalali and Ost-
ovarzadeh 2009).
Sheep manure extract
Sheep manure was collected from the University farm in
Hamedan. Sheep manure extraction was made by stirring
50 g of dry sheep manure (sieved to 2 mm) in 1.0 l
deionized water. The suspension was stirred for 2 h, cen-
trifuged for 20 min, and filtered through Whatman 42 filter
paper. After adjusting the pH to 7.0 with 1 M NaOH, this
solution was used for only 1 week while being stored 4�C.
The K concentration of the SME was analyzed by flame
photometer.
Leaching experiments
The leaching columns consisted of Pyrex tubes, 30-cm
long; with an inner diameter of 4.9 cm. Columns were
filled with soil to a height of 20 cm by uniform tapping to
achieve a uniform bulk density of 1.3–1.4 g cm-3. During
packing each soil was funneled into columns, while the
walls were being simultaneously tapped with a wood rod to
achieve a uniform packing at the same bulk density.
A Whatman No. 42 filter paper was placed at the bottom of
the leaching column (Jalali and Ostovarzadeh 2009). The
bottom of the column was covered with nylon mesh. The
solution was pounded (about 5 cm above the soil surface)
on the soil column, and maintained during the leaching
process. A filter paper was placed on the soil surface to
minimize soil disturbance from the addition of leaching
solution. Then, soil columns were leached with H2O,
0.01 M CaCl2, 0.01 M EDTA, and SME (each solution
was applied only in one column). Leachates were collected
in 0.2 pore volumes (PV) increments and after 3 PV in
0.5–1 PV increments. Porosity is the volume of soil voids
(pore space). The proportion of the soil occupied by water
and air is referred to as the pore volume. It is expressed in
relation to the bulk volume of the soil. The water holding
capacity of a soil depends on its porosity, and the size
distribution of its pores. Pore volume is that part of soil not
occupied by the soil matrix. In the field, without the soil
saturation, the PV is filled partly with soil air and partly
with soil water. In leaching columns, the PV is filled
entirely by the soil water. The pore volume of soil columns
was calculated from the value of the bulk density and
particle density (2.65 g cm-3) of the soil in the column
(Rowell 1994) to be 178–192 ml (Jalali and Ostovarzadeh
2009). The quantity of K leached was calculated using the
concentrations of K and the volume of leachate fraction.
The study was conducted in two replicates at room tem-
perature (22–24�C). Duplicate columns for each soil were
observed to give identical patterns of K leaching. To
simulate the long-term leaching of K, the leaching column
was left until 15 PV was leached from the soils.
Results and discussion
Leaching of K from soils
The results of the leaching are presented as breakthrough
curves (Figs. 1, 2, 3, 4). In all treatments, the two sides of
the breakthrough curves have different characteristics.
Movement of K in soil is affected markedly by its extent of
sorption by the soil. Chemical processes can influence
sorption reaction, control the concentration of K in solu-
tion, and their transport through the soil profile.
In soil leached with SME, leaching of K was small, with
a steady decrease in K concentration as the experiments
proceed (Fig. 1). In soil 1, the maximum K concentration
(312 mg l-1) was observed for about 0.6 PV, after which
the concentration of K decreased rapidly with a long tail
from 23 to 70 mg l-1 during the rest of the percolation.
These concentrations of K in the SME leachate were higher
than the drinking water standard which is 12 mg l-1
(WHO 1993). In other three soils, concentration of K in the
leachate was very lower than soil 1. Exchangeable and
solution forms are primarily involved in leaching (Kolah-
chi and Jalali 2007). The available K (exchangeable and
solution K) in the contaminated soils used for this study, as
extracted by 1 M NH4OAc was 420–920 mg kg-1. Table 1
shows the total amounts leached in 2 and 9.5 PV and
percent of available K leached from soils. In the SME
treatment, the leaching was stopped after 9.5 PV. The
amount leached varied from 1.4 to 241 kg ha-1 and 5 to
576 kg ha-1 after 2 and 9.5 PV had passed through the
column, respectively. Concentration of K in SME was
286 mg l-1 and about 503–824 mg K column-1 was
added to the soils during the experiment. Thus, the amounts
leached were less than the amount added through the SME,
indicating that some K was retained by the soil. Li and
Shuman (1996) stated that these results probably were due
Environ Earth Sci (2012) 66:31–37 33
123
to preliminary sorption of organic ligands on to the soil
with the creation of new sorbing surfaces. The SME
probably released exchangeable forms of K, but the
retention of the dissolved organic matter by the soil may
have provided more active sites to adsorb K or K-organic
complexes on soil surfaces. Jalali and Ranjbar (2009)
Sheep manure extract
0
0.5
1
1.5
2
2.5
3
3.5
4
4.5
0 1 2 3 4 5 6 7 8 9 10
Pore volumes
K (
mg
l-1)
(so
il 2-
4)0
50
100
150
200
250
300
350
K (
mg
l-1)
(so
il 1)
Soil 2 Soil 3 Soil 4 Soil 1
Fig. 1 Breakthrough curves for
K leached with sheep manure
extract in the four contaminated
soils
EDTA
0
5
10
15
20
25
30
35
0 2 4 6 8 10 12 14 16
Pore volumes
K (
mg
l-1)
(so
il 2-
4)
0
500
1000
1500
2000
2500
3000
3500
K (
mg
l-1)
(so
il 1)
Soil 2 Soil 3 Soil 4 Soil 1
Fig. 2 Breakthrough curves for
K leached with 10 mM EDTA
in the four contaminated soils
CaCl2
0
5
10
15
20
25
30
35
40
0 2 4 6 8 10 12 14 16
Pore volumes
K (
mg
l-1)
(so
il 2-
4)
0
500
1000
1500
2000
2500
3000
3500
4000
K (
mg
l-1)
(so
il 1)
Soil 2 Soil 3 Soil 4 Soil 1
Fig. 3 Breakthrough curves for
K leached with 10 mM CaCl2 in
the four contaminated soils
34 Environ Earth Sci (2012) 66:31–37
123
studied effects of sodic water on nutrient leaching in
poultry and sheep manure amended soils. They indicated
that the application of sheep and poultry manure to soils
caused an increase in cation exchange capacity and
adsorption of K. Petruzzelli (1989) also showed that the
addition of sewage sludge extract increased the amount of
heavy metals retained by soil.
The leaching of K by 0.01 M EDTA is shown in Fig. 2.
The maximum K concentration (3,313 mg l-1) was
observed for about 0.2 PV followed by decrease in the
subsequent fractions in soil 1. In other three soils, con-
centration of K in the leachate was very lower than soil 1.
In soil 4, concentration of K in the leachate remained
higher than the drinking water standard through the
experiment. Potassium leaching is affected by soil texture
and available K (Rosolem et al. 2010; Evangelou and
Lumbaraja 2002), among other factors. The high available
K content of soil 1 may result in increases of the leaching
of K as compared to the other soils. The amount leached
varied from 0.13 to 49.1% and 0.75 to 56.6% of the
extractable K after 2 and 15 PV had passed through the
column, respectively (Table 1). In this treatment, it seems
that a leaching process had been brought on by increased
ion-exchange of K and release from soils by ambient cat-
ions introduced with the EDTA. The leaching of K by the
0.01 M EDTA was larger than that for the SME, indicating
Distilled
0
5
10
15
20
25
30
35
40
45
0 2 4 6 8 10 12 14 16
Pore volumes
K (
mg
l-1)
(so
il 2-
4)0
200
400
600
800
1000
1200
1400
K (
mg
l-1)
(so
il 1)
Soil 2 Soil 3 Soil 4 Soil 1
Fig. 4 Breakthrough curves for
K leached with distilled water in
the four contaminated soils
Table 1 Amounts of K leached
from column of soils
a In case of SME amount
leached after 9.5 pore volumes
Soil No. Treatments Amount leached in 2 PV Amount leached in 15 PVa
kg ha-1 % of
exchangeable K
kg ha-1 % of
exchangeable K
1 SME 241 – 576 –
EDTA 954 49.1 1081 56.6
CaCl2 1134 59.3 1249 65.3
DW 595 31.2 676 35.4
2 SME 2.3 – 8 –
EDTA 19 1.1 120 6.4
CaCl2 25 1.4 116 6.2
DW 19 1.1 51 2.7
3 SME 1.4 – 5 –
EDTA 5.9 0.13 33 0.75
CaCl2 7.6 0.17 28 0.62
DW 8.6 0.2 21 0.5
4 SME 4.7 – 22 –
EDTA 49.3 5.2 349 37.3
CaCl2 54.1 5.8 387 41.3
DW 43 4.6 139 14.9
Environ Earth Sci (2012) 66:31–37 35
123
a high potential of EDTA to solubilize K in the soil. These
results suggest that EDTA is a potential agent to remove K
from metal-contaminated soil.
The curved pattern for leached K from 0.01 M CaCl2was approximately similar to the 0.01 M EDTA, whereas
the leaching with 0.01 M CaCl2 was relatively higher at the
first pore volume (Fig. 3). The amount leached varied from
0.17 to 59.3% and 0.62 to 65.3% of the extractable K after
2 and 15 PV had passed through the column, respectively
(Table 1). The K concentrations in the leachate varied from
22 to 35 mg K l-1 for soil 4. These concentrations are
greater than the recommended guideline of the World
Health Organization (12 K mg l-1) (WHO 1993).
Jalali and Rowell (2003) stated that a large amount of
Ca in the CaCl2 can displace K from adsorption sites on the
soil solids. The total amount leached by 0.01 M CaCl2 was
greater than that leached by SME (Table 1) and approxi-
mately similar to the amount leached by EDTA. The results
show that contaminated soils which are irrigated with
Ca-rich water can lose large amounts of K, ranging from 28
to 1249 kg ha-1 for 15 PV. In the uncontaminated soil
leached with 0.01 M CaCl2, Kolahchi and Jalali (2007)
found that 198–388 kg ha-1 was leached with 20 PV.
Because cation exchange is the most important mecha-
nisms that affect K mobility, CaCl2 was represented as
exchange-solution. This solution is considered to simulate
soil pore water in calcareous soils (Shuman 1990; Robbins
et al. 1999). They indicated that 0.01 M CaCl2 has com-
parable ionic strength to natural soil solutions, thus the
leachability of CaCl2 should be similar to that for the
natural soil solution. In addition, in the studied area Ca is
the dominant ion in wells water, representing on average
43.6% of all cations (Jalali 2002). Its concentration in
irrigation water varies from 0.01 to 11.3 mM.
Figure 4 shows the breakthrough curves for an experi-
ment involving the leaching of K with distilled water. The
peak concentration of K recovered after 0.2 PV and then
decreased. The concentration of K in the leachate of dis-
tilled water was high, especially at the beginning of the
leaching period (16–1200 mg l-1) and then decreased and
was less than 12 mg l-1 after four PV in all studied soils.
The amount leached varied from 0.5% (21 kg ha-1) to
35.4% (676 kg ha-1) of the extractable K after 15 PV had
passed through the column (Table 1). In this experiment, it
can be expected that the leaching of K be less than other
leaching solutions, because the supply of cations able to
exchange with K was limited. In the uncontaminated soil
leached with distilled water, Kolahchi and Jalali (2007)
found that 19 (5.7% extractable K) and 61 (18.4%
extractable K) kg ha-1 were leached with 5 and 20 PV,
respectively. The higher amounts leached here may be due
to the higher extractable K and CaCO3 in the studied soils.
Carbonate calcium dissolution is the main source of Ca for
displacing other cations from exchange sites (Kolahchi and
Jalali 2007). The soils contain CaCO3 (138–185 g kg-1)
that can solubilize to supply Ca to replace K ions. In the
field, the release of CO2 in the root zone increases CaCO3
dissolution.
The forms of K in soil, in order of their availability for
leaching, are solution, exchangeable, non-exchangeable
and mineral (Martin and Sparks 1985; Sparks and Huang
1985). Exchangeable and solution forms are primarily
involved in leaching. At the end of leaching experiments
with all leaching solutions, the extractable K (NH4OAc-K)
was not yet leached and total K leached (Table 1) is less
than NH4OAc-K and so measured K leached is mainly
influenced by K availability in these contaminated soils.
Therefore, land application of sheep manure can
increase the levels of soluble and exchangeable forms of K.
Sheep manure application not only increases these forms of
K, but also the organic matter of the soil and in turn and its
cation exchange capacity. The potential for accumulation
of K in soil from sheep manure application is high since the
K has a low leachability. Potassium ions are adsorbed by
the soil particles and organic matter provided by sheep
manure and thus minimizing the risk of potassium
leaching.
However, the column leaching experiment was not a
perfect simulation of the field situation. But column studies
have frequently been used to provide information about
element release and transport in soil (Camobreco et al.
1996; Rowell 1994; Jalali and Rowell 2003; Voegelin et al.
2003; Qureshi et al. 2004), and may, therefore constitute an
adequate tool for the achievement of the K leaching.
Conclusions
Application of EDTA and SME in reclamation of con-
taminated soils may also cause leaching of nutrients,
including K. To better understand K leaching by EDTA
and SME and its contribution to poor water quality, soil
columns were employed to investigate the movement of K
in some contaminated calcareous soils. The leaching of K
by the 0.01 M EDTA was larger than that for the SME,
indicating a high potential of EDTA to solubilize K in these
contaminated calcareous soils. These results suggest that
EDTA is a potential agent to remove K from metal-con-
taminated soil. Sheep manure by supplying nutrients, par-
ticularly K, can improve the mineral nutrient status and
growth of plants grown in such soils. In addition, appli-
cation of Ca-rich water in reclamation of contaminated
soils may also cause leaching of K. Therefore, an increase
in the K concentration can be expected in groundwater
within infiltration areas. Such increases can even lead to a
breach of the drinking water limit for K (12 mg l-1).
36 Environ Earth Sci (2012) 66:31–37
123
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